Halogen-Substituted Pyrazole Synthesis via Piperazine Derivatives

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Solution Overview

Problem

Current methods for synthesizing halogen-substituted pyrazole derivatives, such as 3-difluoromethyl-1-methylpyrazole-4-carboxylic acid, face challenges including high costs, environmental concerns, harsh reaction conditions, and selectivity issues, making them unsuitable for industrial production.

Innovation Solution

A method involving a piperazine derivative reacting with a halogenated acetyl halide derivative in chloroform, using triethylamine as a catalyst, followed by ring closure with methylhydrazine and subsequent hydrolysis or oxidation to produce halogen-substituted pyrazole compounds, optimizing the reaction route for high yield and purity.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If the Claisen condensation method is used to synthesize 3-difluoromethyl-1-methylpyrazole-4-carboxylic acid, then the product can be obtained through established reaction steps, but the production cost becomes excessively high

Engineering Contradiction:
Improveproduct obtainabilityVSAvoidproduction cost
Core Design Contradiction:
ReliabilityVSEase of manufacture

Solution Approach 1:

The invention changes the chemical parameters by using difluoroacetyl chloride instead of ethyl difluoroacetate as the starting material. This parameter change in the reactant structure leads to a more cost-effective synthesis route while maintaining product obtainability through the same pyrazole ring formation mechanism

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The invention extracts and eliminates the costly Claisen condensation step from the synthesis route. By directly reacting difluoroacetyl chloride with vinyl ether and then with methylhydrazine, the method removes the intermediate ethyl difluoroacetoacetate formation step, thereby reducing production costs while still achieving reliable product synthesis

Inventive Principle:
Principle #2Taking out (Extraction)

2Productivity

If dimethylaminoethyl acrylate method is used, then the synthesis route becomes shorter with higher yield, but equipment requirements increase and environmental pollution occurs due to volatile dimethylamine

Engineering Contradiction:
Improvesynthesis efficiencyVSAvoidenvironmental pollution
Core Design Contradiction:
ProductivityVSObject-affected harmful factors

Solution Approach 1:

The invention replaces the expensive and environmentally problematic dimethylaminoethyl acrylate with a simpler, more economical approach using vinyl ether and difluoroacetyl chloride. This substitution uses cheaper, less hazardous materials that do not generate volatile amine pollutants, while maintaining high synthesis efficiency through direct reaction pathways

Inventive Principle:
Principle #27Cheap short-living objects (Disposable)

Solution Approach 2:

The invention converts the potential harm of using complex reagents into a benefit by selecting materials that are both efficient and environmentally friendly. The use of difluoroacetyl chloride and vinyl ether avoids the generation of volatile dimethylamine, transforming the synthesis process into one that is both productive and environmentally acceptable

Inventive Principle:
Principle #22Blessing in disguise (Convert harm into benefit)

3Ease of manufacture

If difluorochloroacetyl chloride method is used, then the reaction can proceed through available reagents, but the synthesis route becomes longer with increased three wastes

Engineering Contradiction:
Improvereagent availabilityVSAvoidwaste generation
Core Design Contradiction:
Ease of manufactureVSLoss of substance

Solution Approach 1:

The invention extracts and removes the unnecessary dechlorination step from the synthesis route. By using difluoroacetyl chloride directly without introducing additional chlorine atoms, the method eliminates the need for zinc powder or palladium catalyst dechlorination steps, thereby reducing both process complexity and waste generation while maintaining reagent availability

Inventive Principle:
Principle #2Taking out (Extraction)

Solution Approach 2:

The invention ensures continuous useful action by designing a synthesis route where each step directly contributes to product formation without requiring additional purification or dechlorination steps. The reaction sequence from difluoroacetyl chloride through vinyl ether to pyrazole derivative maintains continuous productivity while minimizing waste

Inventive Principle:
Principle #20Continuity of useful action

4Ease of manufacture

If other synthesis methods such as dichloroacetyl chloride method are used, then cost control may be achieved, but reaction conditions become harsh with difficult operation and isomer separation

Engineering Contradiction:
Improvecost controlVSAvoidoperation convenience
Core Design Contradiction:
Ease of manufactureVSEase of operation

Solution Approach 1:

The invention changes the reaction parameters by using difluoroacetyl chloride instead of dichloroacetyl chloride, which allows milder reaction conditions. This parameter change in the starting material eliminates the need for harsh conditions like -40 to -20°C and constant pressure changes, thereby improving operational convenience while maintaining cost-effectiveness through a streamlined synthesis route

Inventive Principle:
Principle #35Parameter changes

Applied Scientific Principles

This section explains which scientific principles are used to turn an abstract innovation direction into a practical engineering solution.

Function Achieved in This Case

This method provides a cost-effective, environmentally friendly, and efficient synthesis of halogen-substituted pyrazole derivatives with high yield and purity, reducing by-products and simplifying the reaction process, while allowing for easy purification and recycling of raw materials.

Implementation Method 1

using triethylamine as a catalyst

Methodology Applied
Scientific EffectCatalysis: Catalysis

Implementation Method 2

reacts with methylhydrazine to close a pyrazole ring

Methodology Applied
Scientific EffectChemical Bonding: Chemical Bonding

Implementation Method 3

subsequent hydrolysis or oxidation to produce halogen-substituted pyrazole compounds

Methodology Applied
Scientific EffectHydrolysis: Hydrolysis

Data Source

PatentEP4008715B1Halogen substituted compound, and preparation method therefor and application thereof
Publication Date: 2024.03.06 SUQIAN KEYLAB BIOCHEMICAL CO LTD
  • EP4008715B1 patent drawingFigure 1
  • EP4008715B1 patent drawingFigure 2
  • EP4008715B1 patent drawingFigure 3

AI summary

The present invention relates to a preparation method for a halogen-substituted compound, where a piperazine derivative shown in formula I reacts with a halogenated acetyl halide derivative shown in formula VI to generate a halogen-substituted compound shown in formula II. The present invention further relates to a preparation method for preparing a pyrazole derivative by using a halogen-substituted compound, where a halogen-substituted compound shown in formula II reacts with methylhydrazine to close a pyrazole ring, to generate a halogen-substituted alkyl-1-methylpyrazole derivative shown in formula IV, or reacts with methylhydrazine benzaldehyde hydrazone to generate a hydrazone compound shown in formula III, which closes, under the action of an acid, a pyrazole ring to generate a halogen-substituted alkyl-1-methylpyrazole derivative shown in formula IV The present invention further relates to a structure of an intermediate compound. The preparation methods for a halogen-substituted compound and a pyrazole derivative of the present invention are suitable for industrial production.